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Annual Meeting Optical Society of America

Nonlinear optical properties of spatially distributed particle composites

Charles M. Bowden

Published Jan 1, 1987• 0 citations
Publisher

Abstract

We examine the nonlinear dielectric response of small spherical grains ϵ m embedded in a linear dielectric ϵ d . The models for the spherical grains are a Kerr medium1,2 and a two-level system.3 The expression for the dielectric function ϵ m is dependent of the grain size; in addition it also depends on the local electric field E L . This field is related to the external applied field E0 by the equation E L = (3ϵ d /ϵ m + 2ϵ d )E0. The steady-state equation for the averaged external field is ∇2E0 + (ω2/c2)ϵ*E0 = 0, where ω is the frequency of the field, ϵ* is the dielectric function from the effective medium approximation, and it is obtained from the self-consistency relation4 〈ϵ(r) − ϵ*/ϵ(r) + 2ϵ*〉 = 0; the angular brackets denote an average taken over the ensemble of dielectric spheres distributed in a small volume. Using the slowly varying-envelope approximation we solve these equations for a distribution of grain radii and the affect this has on the effective optical nonlinearities. In particular, we show its effect on the optical bistability for these composite systems.

DOI
10.1364/oam.1987.tud7

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We examine the nonlinear dielectric response of small spherical grains ϵ m embedded in a linear dielectric ϵ d . The models for the spherical grains are a Kerr medium1,2 and a two-level system.3 The expression for the dielectric function ϵ m is dependent of the grain size; in addition it also depends on the local electric field E L . This field is related to the external applied field E0 by the equation E L = (3ϵ d /ϵ m + 2ϵ d )E0. The steady-state equation for the averaged external field is ∇2E0 + (ω2/c2)ϵE0 = 0, where ω is the frequency of the field, ϵ is the dielectric function from the effective medium approximation, and it is obtained from the self-consistency relation4 〈ϵ(r) − ϵ*/ϵ(r) + 2ϵ*〉 = 0; the angular brackets denote an average taken over the ensemble of dielectric spheres distributed in a small volume. Using the slowly varying-envelope approximation we solve these equations for a distribution of grain radii and the affect this has on the effective optical nonlinearities. In particular, we show its effect on the optical bistability for these composite systems.
Nonlinear optical properties of microstructures immersed in a linear dielectric are investigated. The microstructures are assumed to be composed of simple saturable two-level atoms. The local field corrections are included in a self-consistent manner leading to multiple solutions for the absorptive part of the dielectric constant of the microstructure as noted earlier by Chemla and Miller.1 For a given structure we use the effective medium theory and average over the random positions of the grains to obtain the effective medium dielectric constant in the quasistatic limit (λ ≪ grain size) as a function of the volume fraction of the grains. The results exhibit sharp hysteresis effects. However, in the study of the propagation in the medium these effects are modified considerably. While defined switches are observed in the mean field at certain points in the medium where the absorption jumps from the upper to lower branch, the optical intensity undergoes only a change of slope.
An effective-medium theory for nonlinear spherical particles embedded in a linear host medium is developed. The formulation is based on a T-matrix approach. Introduction of a field-dependent T matrix enables one to obtain an exact expression for effective dielectric constant of a medium with spherical grains. In the special cases of low-field values, the results obtained previously for the third- and fifth-order nonlinear susceptibilities of the medium are recovered. The resonance behavior of the effective dielectric constant and intrinsic optical bistability are also discussed.
We studied the intrinsic optical bistability(OB) of coated spherical particles with graded dielectric profiles.According to Maxwell equations, we obtained the spatial average of the local field in the core as a function of the external applied field. Numerical results for power-law graded profiles show that the optical bistable behavior is dependent on the shell thickness and the power-laws exponent k. The interval of optical bistability increases with increasing shell thickness or increasing k. In addition, the field-dependent reflectance at normal incidence R in random composites is also investigated, and a hysteretic loop is observed.
Abstract Optically bistable behaviour is demonstrated for systems consisting of optically nonlinear microcrystallites embedded in an optically linear metal or dielectric. The most simple version of the local‐field correction serves as feedback mechanism thus avoiding external mirrors. The dielectric function for macroscopic samples is calculated with Garnett's effective medium theory. Numerical examples for the reflectivity and the transmissivity are given for an embedded dielectric with exciton‐like nonlinearity.
The propagation of electromagnetic waves in a nonlinear medium composed of semiconductor microcrystallites embedded in a host medium has been investigated. Explicit results are given for the case of cadmium sulfide grains in glass when a saturable two-level approximation is used for the nonlinear dielectric function. The bistable behavior, noticed earlier by Chemla and Miller [ Opt. Lett.11, 522 ( 1986)], for single grains is manifested in the propagation studies conducted here by the occurrence of a discontinuity in the index of refraction in the medium. Various approximations are used to obtain the optical bistability properties. Possible applications of this feature are pointed out.
The intrinsic optical bistability (OB) of graded core-shell granular composites is investigated. The coated particles are made of cores with gradient dielectric function ∊ c (r) = A(r/a) k and nonlinear shells. In view of the exponential distribution of the core dielectric constant, the potential functions of each region are obtained by solving the Maxwell equations, and the mathematical expressions of electric field in the shells and cores are determined. Numerical study reveals that the optical bistable threshold and the threshold width of the composite medium are dependent on the shell thickness, core dielectric exponent, and power function coefficient. The optical bistable width increases with the decreasing shell thickness and the power exponent and with the increasing power function coefficient.